Photocatalytic hydrogen evolution and pollutant degradation are both promising strategies for clean energy production and environmental remediation, yet their integration for synchronous wastewater-to-energy conversion is fundamentally hindered by inefficient charge utilization and severe interfacial redox competition. Herein, a quantum-dot-bridged dual-defect interface engineering strategy is developed to synchronize photocatalytic oxidation and hydrogen evolution for wastewater-to-energy conversion. As a result, a hierarchical S-type heterostructure was constructed by integrating Ti 3 C 2 MXene quantum dots with electron-storage capability, sulfur-vacancy-rich MoS 2 , and oxygen-deficient CeO 2 (TMMC), which effectively accelerated interfacial charge transport. The optimized catalyst achieves a hydrogen evolution rate of 12.17 mmol g -1 h -1 with 98.6% norfloxacin removal and maintains high stability under continuous operation. In pollutant-containing systems, hydrogen production reaches 274.35 μmol g -1 h -1 and further increases to 405.93 μmol g -1 h -1 upon low-dose peroxymonosulfate addition. Mechanistically, Ce-O-Mo interfacial coupling induces asymmetric charge redistribution and a built-in electric field for directional carrier separation, while spatially separated sulfur and oxygen vacancies regulate proton reduction and oxidant activation, respectively, mitigating interfacial redox competition. This work establishes defect-coordinated interfacial engineering as a general paradigm for regulating charge utilization and reaction selectivity in integrated photocatalytic systems. A bifunctional TMMC photocatalyst with excellent photoelectrical properties is developed for the simultaneous oxidation of pollutants and hydrogen evolution under visible light. The corresponding charge-transfer pathway and photocatalytic mechanism are illustrated in TOC figure. • Constructing MXene quantum-dot-mediated dual-vacancy architectures via interfacial engineering. • Enabling spatially decoupled oxidation and reduction through vacancy-guided S-scheme charge transfer. • Boosting H 2 production to 405.93 μmol g -1 h -1 alongside 98.6% norfloxacin removal via low PMS addition. • Establishing a photo-Fenton-like platform integrating advanced oxidation with hydrogen recovery. • LCA confirms reduced environmental burdens and costs for sustainable wastewater-to-energy conversion.
Zhu et al. (Fri,) studied this question.